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• W4313487949 endingPage "821" @default.
• W4313487949 startingPage "811" @default.
• W4313487949 abstract "The catalytic transformation of N2 to NH3 by transition metal complexes is of great interest and importance but has remained a challenge to date. Despite the essential role of vanadium in biological N2 fixation, well-defined vanadium complexes that can catalyze the conversion of N2 to NH3 are scarce. In particular, a V(NxHy) intermediate derived from proton/electron transfer reactions of coordinated N2 remains unknown. Here, we report a dinitrogen-bridged divanadium complex bearing POCOP (2,6-(tBu2PO)2-C6H3) pincer and aryloxy ligands, which can serve as a catalyst for the reduction of N2 to NH3 and N2H4. Low-temperature protonation and reduction of the dinitrogen complex afforded the first structurally characterized neutral metal hydrazido(2−) species ([V]═NNH2), which mediated 15N2 conversion to 15NH3, indicating that it is a plausible intermediate of the catalysis. DFT calculations showed that the vanadium hydrazido complex [V]═NNH2 possessed a N–H bond dissociation free energy (BDFEN–H) of as high as 59.1 kcal/mol. The protonation of a vanadium amide complex ([V]–NH2) with [Ph2NH2][OTf] resulted in the release of NH3 and the formation of a vanadium triflate complex, which upon reduction under N2 afforded the vanadium dinitrogen complex. These transformations model the final steps of a vanadium-catalyzed N2 reduction cycle. Both experimental and theoretical studies suggest that the catalytic reaction may proceed via a distal pathway to liberate NH3. These findings provide unprecedented insights into the mechanism of N2 reduction related to FeV nitrogenase." @default.
• W4313487949 created "2023-01-06" @default.
• W4313487949 creator A5003934555 @default.
• W4313487949 creator A5004243344 @default.
• W4313487949 creator A5009439958 @default.
• W4313487949 creator A5011003735 @default.
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• W4313487949 creator A5027464301 @default.
• W4313487949 creator A5060105914 @default.
• W4313487949 creator A5087674282 @default.
• W4313487949 creator A5088871411 @default.
• W4313487949 date "2023-01-03" @default.
• W4313487949 modified "2023-10-09" @default.
• W4313487949 title "Vanadium-Catalyzed Dinitrogen Reduction to Ammonia via a [V]═NNH₂ Intermediate" @default.
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